Direct Observation of Ultrafast Exciton Formation in a Monolayer of WSe2

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Philipp Steinleitner - , University of Regensburg (Author)
  • Philipp Merkl - , University of Regensburg (Author)
  • Philipp Nagler - , University of Regensburg (Author)
  • Joshua Mornhinweg - , University of Regensburg (Author)
  • Christian Schüller - , University of Regensburg (Author)
  • Tobias Korn - , University of Regensburg (Author)
  • Alexey Chernikov - , University of Regensburg (Author)
  • Rupert Huber - , University of Regensburg (Author)

Abstract

Many of the fundamental optical and electronic properties of atomically thin transition metal dichalcogenides are dominated by strong Coulomb interactions between electrons and holes, forming tightly bound atom-like states called excitons. Here, we directly trace the ultrafast formation of excitons by monitoring the absolute densities of bound and unbound electron-hole pairs in single monolayers of WSe2 on a diamond substrate following femtosecond nonresonant optical excitation. To this end, phase-locked mid-infrared probe pulses and field-sensitive electro-optic sampling are used to map out the full complex-valued optical conductivity of the nonequilibrium system and to discern the hallmark low-energy responses of bound and unbound pairs. While the spectral shape of the infrared response immediately after above-bandgap injection is dominated by free charge carriers, up to 60% of the electron-hole pairs are bound into excitons already on a subpicosecond time scale, evidencing extremely fast and efficient exciton formation. During the subsequent recombination phase, we still find a large density of free carriers in addition to excitons, indicating a nonequilibrium state of the photoexcited electron-hole system.

Details

Original languageEnglish
Pages (from-to)1455-1460
Number of pages6
JournalNano letters
Volume17
Issue number3
Publication statusPublished - 8 Mar 2017
Peer-reviewedYes
Externally publishedYes

External IDs

PubMed 28182430

Keywords

Keywords

  • atomically thin 2D crystals, Dichalcogenides, exciton formation, ultrafast dynamics